Abstract

The electrochemical splitting of water holds promise for the storage of energy produced intermittently by renewable energy sources. The evolution of hydrogen currently relies on the use of platinum as a catalyst—which is scarce and expensive—and ongoing research is focused towards finding cheaper alternatives. In this context, 2D polymers grown as single layers on surfaces have emerged as porous materials with tunable chemical and electronic structures that can be used for improving the catalytic activity of metal surfaces. Here, we use designed organic molecules to fabricate covalent 2D architectures by an Ullmann‐type coupling reaction on Au(111). The polymer‐patterned gold electrode exhibits a hydrogen evolution reaction activity up to three times higher than that of bare gold. Through rational design of the polymer on the molecular level we engineered hydrogen evolution activity by an approach that can be easily extended to other electrocatalytic reactions.

Highlights

  • The 2D porous single-layer polymer is structurally similar to the organic sheets that build up 2D covalent organic frameworks (COFs)

  • COFs have recently emerged as active photocatalysts for hydrogen production,[10,11,12] whereby the organic frameworks can efficiently absorb light as a result of their suitable band gaps

  • It is noteworthy that exposure of P-N3 to the electrolyte without applying any potential already leads to the appearance of a peak at 400 eV, indicative of the interaction of water with the polymer. From this observation we can infer that the nitrogen atoms in the polymer act as interaction sites for water molecules, which stabilize H2O close to the gold electrode

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Summary

Introduction

We use scanning tunneling potential window À0.70 to À0.95 VAg/AgCl which are not microscopy (STM), X-ray photoelectron spectroscopy (XPS), present from the bare Au(111) surface (see the Supporting electrochemical (EC) measurements, and density functional Information for further discussion). From this observation we can infer that the nitrogen atoms in the polymer act as interaction sites for water molecules, which stabilize H2O close to the gold electrode.

Results
Conclusion

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